A high-quality perovskite film with interconnected perovskite grains was obtained by incorporating terephthalic acid (TPA) additive into the perovskite precursor solution. The presence of TPA changed the crystallization kinetics of the perovskite film and promoted lateral growth of grains in the vicinity of crystal boundaries. As a result, sheet-shaped perovskite was formed and covered onto the bottom grains, which made some adjacent grains partly merge together to form grains-interconnected perovskite film. Perovskite solar cells (PSCs) with TPA additive exhibited a power conversion efficiency (PCE) of 18.51% with less hysteresis, which is obviously higher than that of pristine cells (15.53%). PSCs without and with TPA additive retain 18 and 51% of the initial PCE value, respectively, aging for 35 days exposed to relative humidity 30% in air without encapsulation. Furthermore, MAPbI film with TPA additive shows superior thermal stability to the pristine one under 100 °C baking. The results indicate that the presence of TPA in perovskite film can greatly improve the performance of PSCs as well as their moisture resistance and thermal stability.

Planar perovskite solar cells (PSCs) that use nickel oxide (NiO) as a hole transport layer have recently attracted tremendous attention because of their excellent photovoltaic efficiencies and simple fabrication. However, the electrical conductivity of NiO and the interface contact properties of the NiO/perovskite layer are always limited for the NiO layer fabricated at a relatively low annealing temperature. Ferrocenedicarboxylic acid (FDA) was firstly introduced to modify a p-type NiO hole transport layer in PSCs, which obviously improves the crystallization of the perovskite layer and hole transport and collection abilities and reduces carrier recombination. PSCs with a FDA modified NiO layer reached a PCE of 18.20%, which is much higher than the PCE (15.13%) of reference PSCs. Furthermore, PSCs with a FDA interfacial modification layer show better UV durability and a hysteresis-free effect and still maintain the original PCE value of 49.8%after being exposed to UV for 24 h. The enhanced performance of the PSCs is attributed to better crystallization of the perovskite layer, the passivation effect of FDA, superior interface contact at the NiO/perovskite layers and enhancement of the electrical conductivity of the FDA modified NiO layer. In addition, PSCs with FDA inserted at the interface of the perovskite/PCBM layers can also improve the PCE to 16.62%, indicating that FDA have dual functions to modify p-type and n-type carrier transporting layers.

Hole transport layer NiOx-based inverted perovskite solar cells (PSCs) have advantages of simple fabrication, low temperature, and low cost. Furthermore, the p-type NiOx material compared to that of typical n-type SnOx for PSCs has better photostability potential due to its lower photocatalytic ability. However, the NiOx layer modified by some typical materials show relatively simple functions, which limit the synthesized performance of NiOx-based inverted PSCs. Phenethyl ammonium iodide (PEAI) was introduced to modify the NiOx/perovskite interface, which can synchronously contribute to better crystallinity and stability of the perovskite layer, passivating interface defects, formed quasi-two-dimensional PEA2PbI4 perovskite layers, and superior interface contact properties. The PCEs of PSCs with the PEAI-modified NiOx/perovskite interface was obviously increased from 20.31 from 16.54% compared to that of the reference PSCs. The PSCs with PEAI modification remained 75 and 72% of the original PCE values aging for 10 h at 85 °C and 65 days in a relative humidity of 15%, which are superior to the original PCE values (47 and 51%, respectively) for the reference PSCs. Therefore, PSCs with the PEAI-modified NiOx/perovskite interface show higher PCEs and better thermal stability and moisture resistance.

As a hole transport layer, PEDOT:PSS usually limits the stability and efficiency of perovskite solar cells (PSCs) due to its hygroscopic nature and inability to block electrons. Here, a graphene-oxide (GO)-modified PEDOT:PSS hole transport layer was fabricated by spin-coating a GO solution onto the PEDOT:PSS surface. PSCs fabricated on a GO-modified PEDOT:PSS layer exhibited a power conversion efficiency (PCE) of 15.34%, which is higher than 11.90% of PSCs with the PEDOT:PSS layer. Furthermore, the stability of the PSCs was significantly improved, with the PCE remaining at 83.5% of the initial PCE values after aging for 39 days in air. The hygroscopic PSS material at the PEDOT:PSS surface was partly removed during spin-coating with the GO solution, which improves the moisture resistance and decreases the contact barrier between the hole transport layer and perovskite layer. The scattered distribution of the GO at the PEDOT:PSS surface exhibits superior wettability, which helps to form a high-quality perovskite layer with better crystallinity and fewer pin holes. Furthermore, the hole extraction selectivity of the GO further inhibits the carrier recombination at the interface between the perovskite and PEDOT:PSS layers. Therefore, the cooperative interactions of these factors greatly improve the light absorption of the perovskite layer, the carrier transport and collection abilities of the PSCs, and especially the stability of the cells. Electronic supplementary materialThe online version of this article (doi:10.1007/s40820-017-0140-x) contains supplementary material, which is available to authorized users.